Individuals facing physical and mental multimorbidity and social marginalization are considered to have “complex health and social needs.” This study seeks to address the following question: what mental health care experiences are valued by individuals with complex health and social needs? Semi-structured interviews were conducted with fifteen individuals experiencing complex health and social needs, including homelessness. Interview data was analyzed using an interpretive description approach. Participants valued services and providers who cared with them and for them. Care for service users with complex needs required flexible processes and individualized care planning and treatment. Care with service users demanded genuine, collaborative interpersonal interactions. These elements were evident across steps in an episode of care, from intake through assessment and treatment to transitions and discharge. These findings highlight particular challenges in operationalizing evidence-based care in mental health care for people with complex health and social needs.